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Herein, we precisely control the type of as\u2010formed ROS by introducing Au single atoms (SAs) on CuO\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    \/ZnO (Au\n                    <jats:sub>1<\/jats:sub>\n                    \u2010CuO\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    \/ZnO), to simultaneously achieve high selectivity and productivity of CH\n                    <jats:sub>3<\/jats:sub>\n                    OH in POM. In situ characterizations and theoretical calculations revealed that the introduced Au SAs significantly altered the electronic structure of Cu atoms, leading to an energy level rearrangement of Cu 3d orbital and the upshift of d\u2010band center, which increased the energy levels of bonding and antibonding states of Au\n                    <jats:sub>1<\/jats:sub>\n                    \u2010CuO\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    \/ZnO\u2010*OOH. Thus, the hybridization between Cu active sites and the key intermediate *OOH was significantly enhanced, especially for the orbital hybridizations of d\n                    <jats:italic>\n                      <jats:sub>z<\/jats:sub>\n                    <\/jats:italic>\n                    <jats:sup>2<\/jats:sup>\n                    \u2010p\n                    <jats:italic>\n                      <jats:sub>z<\/jats:sub>\n                    <\/jats:italic>\n                    and d\n                    <jats:italic>\n                      <jats:sub>xz<\/jats:sub>\n                    <\/jats:italic>\n                    \/d\n                    <jats:italic>\n                      <jats:sub>yz<\/jats:sub>\n                    <\/jats:italic>\n                    \u2010p\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    . This facilitated the dissociation of O\u2500O to form *OH intermediate rather than the direct desorption of *OOH, thereby ultimately determining the ROS type in aerobic POM. Additionally, the asymmetric electronic structure of Au\n                    <jats:sub>1<\/jats:sub>\n                    \u2010CuO\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    \/ZnO could also lower the first C\u2013H dissociation energy by structural polarization of CH\n                    <jats:sub>4<\/jats:sub>\n                    molecules. As a result, Au\n                    <jats:sub>1<\/jats:sub>\n                    \u2010CuO\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    \/ZnO exhibited an excellent CH\n                    <jats:sub>3<\/jats:sub>\n                    OH productivity of 16856\u00a0\u00b5mol\u00b7g\n                    <jats:sub>cat.<\/jats:sub>\n                    <jats:sup>\u22121<\/jats:sup>\n                    with 100% selectivity during POM at mild conditions.\n                  <\/jats:p>","DOI":"10.1002\/anie.202505267","type":"journal-article","created":{"date-parts":[[2025,5,23]],"date-time":"2025-05-23T06:31:17Z","timestamp":1747981877000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":24,"title":["Regulating Reactive Oxygen Species via Orbital Rehybridization Between Intermediate and Active Site for Selective Methane Photooxidation to Methanol"],"prefix":"10.1002","volume":"64","author":[{"given":"Fangyuan","family":"Si","sequence":"first","affiliation":[{"name":"School of Chemistry and Chemical Engineering State Key Laboratory of Pulp and Paper Engineering South China University of Technology  Guangzhou 510640 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junxian","family":"Bai","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering State Key Laboratory of Pulp and Paper Engineering South China University of Technology  Guangzhou 510640 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yan","family":"Li","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering State Key Laboratory of Pulp and Paper Engineering South China University of Technology  Guangzhou 510640 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ruimin","family":"Lan","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering State Key Laboratory of Pulp and Paper Engineering South China University of Technology  Guangzhou 510640 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shijing","family":"Cheng","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering State Key Laboratory of Pulp and Paper Engineering South China University of Technology  Guangzhou 510640 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tingting","family":"Hou","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering State Key Laboratory of Pulp and Paper Engineering South China University of Technology  Guangzhou 510640 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1527-551X","authenticated-orcid":false,"given":"Yingwei","family":"Li","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering State Key Laboratory of Pulp and Paper Engineering South China University of Technology  Guangzhou 510640 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,6,2]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1002\/advs.202001946"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1039\/D1CS00783A"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.rser.2020.110024"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.trechm.2022.09.003"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.9b11440"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-021-24912-0"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-022-30434-0"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1002\/cssc.202200548"},{"key":"e_1_2_7_9_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.0c09727"},{"key":"e_1_2_7_10_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202202914"},{"key":"e_1_2_7_11_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41560-022-00988-w"},{"key":"e_1_2_7_12_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202303896"},{"key":"e_1_2_7_13_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41929-020-00546-1"},{"key":"e_1_2_7_14_1","volume":"63","author":"Xu Y.","year":"2024","journal-title":"Angew. 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